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Onset and impact of plastic deformation in granular compaction
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Structural mechanism of HP1⍺-dependent transcriptional repression and chromatin compaction
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Sulfate Promotes Compact CaCO 3 Formation and Protects Portland Cement from Supercritical CO 2 Attack
Supercritical (sc) CO 2 in geologic carbon sequestration (GCS) can chemically and mechanically deteriorate wellbore cement, raising concerns for long-term operations. In contrast to the conventional view of “sulfate attack” on cement, we found that adding 0.15 M sulfate to the acidic brine can significantly reduce the impact of scCO 2 attack on Portland cement, resulting in stronger cement than that found in a sulfate-free system. Scanning electron microscopy revealed a decreased total attack depth in reacted cement in the presence of sulfate. With a newly defined minimum porosity term in reactive transport modeling, our model suggests that sulfate caused CaCO 3 to fill more nanopore spaces in the cement. Small angle X-ray scattering experiments also showed that sulfate can decrease the pore sizes of the carbonate layer. The results suggest that the interactions between sulfate and cement can generate a less porous CaCO 3 layer, which better resists acidic brine. Using this mechanism as a proof-of-concept, we tested the incorporation of sodium sulfate into Portland cement and synthesized new cement composites that show stronger resistance against scCO 2 attacks. Finally, these newly discovered interfacial interactions between CaCO 3 and sulfate provide new insights into engineering mechanically strong and green materials for safer GCS.
Physics-Driven Construction of Compact Primitive Gaussian Density Fitting Basis Sets
We present a model-assisted density fitting (MADF) basis set generator, an algorithm for generating primitive atomic Gaussian density fitting (DF) basis sets (DFBSs) from a contracted Gaussian orbital basis set (OBS). The MADF algorithm produces DFBSs suitable for accurate robust DF approximation of 2-particle interactions in mean-field and correlated electronic structures. The algorithm is designed to (a) saturate the OBS product space by a large regularized set of primitive solid-harmonic Gaussian shells with nonuniform distribution of exponents, followed by (b) pruning of the shells according to their contributions to the 2- body energy of a correlated atomic ensemble. Building the DFBS generator model almost exclusively on mathematical and physical principles allows one to limit the number of parameters that control the density fitting error to three, with a single set of parameters sufficient for computations with all basis cardinal numbers, with and without correlation of core electrons, with and without scalar and spin-dependent relativistic effects, spanning almost all of the Periodic Table. Performance assessment included basis sets up to quadruple-ζ quality from several major basis set families, using molecules composed of main-group, d-block, and f-block elements. The resulting DF errors in Hartree−Fock and second-order MP2 energies (with relativistic all-electron treatments, when appropriate) were on the order of 20 and 10 μE h per electron, respectively.
Atomic Alignment in PbS Nanocrystal Superlattices with Compact Inorganic Ligands via Reversible Oriented Attachment of Nanocrystals
Nanocrystals (NCs) serve as versatile building blocks for the creation of functional materials with NC self-assembly offering opportunities to enable novel material properties. Here, in this work, we demonstrate that PbS NCs functionalized with strongly negatively charged metal chalcogenide complex (MCC) ligands, such as Sn 2 S 6 4– and AsS 4 3– , can self-assemble into all-inorganic superlattices with both long-range superlattice translational and atomic-lattice orientational order. Structural characterizations reveal that the NCs adopt an unexpected edge-to-edge alignment, and numerical simulation clarifies that orientational order is thermodynamically stabilized by many-body ion correlations originating from the dense electrolyte. Furthermore, we show that the superlattices of Sn 2 S 6 4– -functionalized PbS NCs can be fully disassembled back into the colloidal state, which is highly unusual for orientationally attached superlattices with atomic-lattice alignment. The reversible oriented attachment of NCs, enabling their dynamic assembly and disassembly into effectively single-crystalline superstructures, offers a pathway toward designing reconfigurable materials with adaptive and controllable electronic and optoelectronic properties.
Structural basis for regulation of CELSR1 by a compact module in its extracellular region
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Material Point Methods Applied to Granular Compaction
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Cryogen-free modular scanning tunneling microscope operating at 4-K in high magnetic field on a compact ultra-high vacuum platform
One of the daunting challenges in modern low temperature scanning tunneling microscopy (STM) is the difficulty of combining atomic resolution with cryogen-free cooling. Further functionality needs, such as ultra-high vacuum (UHV), high magnetic field (HF), and compatibility with μm-sized samples, pose additional challenges to an already ambitious build. We present the design, construction, and performance of a cryogen-free, UHV, low temperature, and high magnetic field system for modular STM operation. An internal vibration isolator reduces vibrations in this system, allowing for atomic resolution STM imaging while maintaining a low base temperature of ∼4 K and magnetic fields up to 9 T. Samples and tips can be conditioned in situ utilizing a heating stage, an ion sputtering gun, an e-beam evaporator, a tip treater, and sample exfoliation. In situ sample and tip exchange and alignment are performed in a connected UHV room temperature stage with optical access. Multisite operation without breaking vacuum is enabled by a unique quick-connect STM head design. A novel low-profile vertical transfer mechanism permits transferring the STM between room temperature and the low temperature cryostat.
A compact x-ray spectrometer for measurements of electron temperature distributions in inertial confinement fusion implosions at OMEGA
The Wedge Range Filter (WRF), commonly used for proton spectroscopy at the OMEGA Laser Facility and National Ignition Facility, is adapted to measure the x-ray continuum spectrum through transmission measurement using a continuous-gradient filter. Continuum x rays emitted from the hotspot of an implosion contain information about the plasma composition and electron temperature. The WRF data are leveraged to probe this distribution, specifically the electron temperature distribution. In this work, the data recorded with the WRF are forward modeled using a temperature distribution model folded with the WRF response function. An uncertainty analysis is conducted through a Bayesian regression algorithm using a Hamiltonian Monte Carlo sampler. This analysis enables the uncertainties in the instrument response to be folded into the uncertainty estimation of the electron temperature and absolute x-ray emission. Data analysis for a series of OMEGA implosions is presented and compared with radiation hydrodynamic simulations.
Compact in situ probe for magnetotransport measurements of 2D materials under variable tensile strain
The recent development of freestanding oxide membranes has opened new opportunities for strain engineering of transition metal oxides beyond values accessible in bulk samples. While a number of studies have been performed with fixed strain, the ability to dynamically control the strain state during measurement would be greatly enabling. To this end, we present an in situ uniaxial strain probe optimized for transport measurements of tensile-strained 2D or quasi-2D materials down to 2 K. Utilizing a flexible polyimide substrate as the stress transfer medium, our platform simplifies the sample preparation process and allows precise alignment of strain fields relative to the crystalline axes. An in situ optical microscope monitors the macroscopic strain state operando and makes it possible to complete an entire magnetotransport study at cryogenic temperatures under continuous strain variations. We demonstrate the capabilities of the probe on a freestanding LaNiO 3 membrane, where we induce tensile strain up to 8% and observe a corresponding strong transport anisotropy. In view of the rapid developments in low-dimensional materials synthesis and the plethora of novel quantum phenomena they exhibit, this strain probe provides general instrumentation for examining and controlling these properties via strain.
Challenges and Opportunities Specific to Microreactors: Compact and Light-Weight Shielding During Operation and Transportation
The problem of designing a shield for a mobile microreactor has been addressed. The principal challenges encountered in this endeavor are the dual goals of increasing radiation protection and decreasing weight. It is recognized that these two goals are contradictory. Increasing shielding naturally increases weight. Conversely, decreasing weight naturally calls for decreasing material inventory, including possibly decreasing shield mass. The operational and regulatory drivers for shielding and transportation constraints are identified and summarized. The main constraints pertain to volume, mass, radiation dose, material feasibility and availability, and decommissioning expectations. The latter are limits on residual contamination and dose rates after the reactor is removed. Progress toward solving the challenge of shielding a transportable microreactor is made by considering a tungsten tetraboride (WB4) shell surrounding the reactor vessel. The shield and a generic microreactor were modeled using the MCNP code. It was determined that the presence of a 16-cm-thick WB4 shield reduces the dose equivalent rate during operations to 3.6 mrem/h just outside of a concrete vault and dome and soil berm surrounding the reactor, which is very near the occupational dose rate limits. Without the WB4 layer, the dose rate at the same location outside the berm would be 120 mrem/h. Most importantly, the presence of the WB4 shield substantially protects the surrounding concrete and soil from activation, thus decreasing the duration of administrative control for the site following removal of the reactor from 16 to 3.4 years. At that point, the site may be decommissioned and returned to unrestricted public access. A limitation on the incorporation of a WB4 shield as an intrinsic component of a microreactor is that it results in a design that is transportable only by using the largest road conveyances and that the load would require special permits for transit through the U.S. highway system. New directions for further improvements and possibly more effective solutions to the shielding problem of a mobile microreactor are discussed in the conclusion section.
The Role of Unit-Cell Topology in Modulating the Compaction Response of Additively Manufactured Cellular Materials using Simulations and Validation Experiments
Additive manufacturing has enabled a transformational ability to create cellular structures (or foams) with tailored topology. Compared to their monolithic polymer counterparts, cellular structures are potentially suitable for systems requiring materials with high specific energy-absorbing capability to provide enhanced damping. In this work, we demonstrate the utility of controlling unit-cell topology with the intent of obtaining a desired stress–strain response and energy density. Using mesoscale simulations that resolve the unit-cell sub-structures, we validate the role of unit-cell topology in selectively activating a buckling mode and thereby modulating the characteristic stress–strain response. Simulations incorporate a linear viscoelastic constitutive model and a hyperelastic model for simulating large deformation of the polymer under both tension and compression. Simulated results for nine different cellular structures are compared with experimental data to gain insights into three different modes of buckling and the corresponding stress–strain response.
A compact approach to higher-resolution resonant inelastic x-ray scattering detection using photoelectrons
The detection of inelastically scattered soft x-rays with high energy resolution usually requires large grating spectrometers. Recently, photoelectron spectrometry for analysis of x-rays (PAX) has been rediscovered for modern spectroscopy experiments at synchrotron light sources. By converting scattered photons to electrons and using an electron energy analyser, the energy resolution for resonant inelastic x-ray scattering (RIXS) becomes decoupled from the x-ray spot size and instrument length. In this work, we develop PAX towards high energy resolution using a modern photoemission spectroscopy setup studying Ba 2 Cu 3 O 4 Cl 2 at the Cu L 3 -edge. We measure a momentum transfer range of 24% of the first Brillouin zone simultaneously. Our results hint at the observation of a magnon excitation below 100 meV energy transfer and show intensity variations related to the dispersion of dd-excitations. With dedicated setups, PAX can complement the best and largest RIXS instruments, while at the same time opening new opportunities to acquire RIXS at a range of momentum transfers simultaneously and combine it with angle-resolved photoemission spectroscopy in a single instrument.
Confronting new NICER mass-radius measurements with phase transition in dense matter and twin compact stars
The (re)analysis of data on the X-ray emitting pulsars PSR J0030+0451 and J0740+6620, as well as new results on PSR J0437-4715 and J1231-1411, are confronted with the predictions of the equation of state (EoS) models allowing for strong first-order phase transition for the mass-radius (M-R) diagram. Here, we use models that are based on a covariant density functional (CDF) EoS for nucleonic matter at low densities and a quark matter EoS, parameterized by the speed of sound, at higher densities. To account for the variations in the ellipses for PSR J0030+0451 obtained from different analyses, we examined three scenarios to assess their consistency with our models, focusing particularly on the potential formation of twin stars. We found that in two scenarios, where the ellipses for PSR J0030+0451 and J0437-4715 with masses close to the canonical mass ∼ 1.4 M ⊙ are significantly separated, our models allow for the presence of twin stars as a natural explanation for potential differences in the radii of these stars.
Using equation of state constraints to classify low-mass compact binary mergers
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Improved moving-puncture techniques for compact binary simulations
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Searching for cosmological stochastic backgrounds by notching out resolvable compact binary foregrounds with next-generation gravitational-wave detectors
Stochastic gravitational-wave backgrounds can be of either cosmological or astrophysical origin. The detection of an astrophysical stochastic gravitational-wave background with ground-based interferometers is expected in the near future. Perhaps even more excitingly, the detection of stochastic backgrounds of cosmological origin by future ground-based interferometers could reveal invaluable information about the early Universe. From this perspective, the astrophysical background is a foreground that can prevent the extraction of this information from the data. In this paper, we revisit a time-frequency domain notching procedure previously proposed to remove the astrophysical foreground in the context of next-generation ground-based detectors, but we consider the more realistic scenario where we remove individually detectable signals by taking into account the uncertainty in the estimation of their parameters. We find that time-frequency domain masks can still efficiently remove the astrophysical foreground and suppress it to about 5% of its original level. Further removal of the foreground formed by unresolvable events (in particular, unresolvable binary neutron stars), which is about 10 times larger than the residual foreground from realistic notching, would require detector sensitivity improvements. Therefore, the main limitation in the search for a cosmological background is the unresolvable foreground itself, and not the residual of the notching procedure.